One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia

Ammonia (NH<sub>3</sub>) plays an irreplaceable role in human life as a promising energy carrier and indispensable chemical raw material. Nitrate electroreduction to ammonium (NRA) not only removes nitrate pollutants, but also can be used for efficient NH<sub>3</sub> producti...

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Main Authors: Kang-Yu Zeng, Jun-Jie Wang, Xiang Fang, Zuo-Xi Li
Format: Article
Language:English
Published: MDPI AG 2022-12-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/12/12/1561
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author Kang-Yu Zeng
Jun-Jie Wang
Xiang Fang
Zuo-Xi Li
author_facet Kang-Yu Zeng
Jun-Jie Wang
Xiang Fang
Zuo-Xi Li
author_sort Kang-Yu Zeng
collection DOAJ
description Ammonia (NH<sub>3</sub>) plays an irreplaceable role in human life as a promising energy carrier and indispensable chemical raw material. Nitrate electroreduction to ammonium (NRA) not only removes nitrate pollutants, but also can be used for efficient NH<sub>3</sub> production under ambient conditions. However, achieving high efficiency and selectivity of electrocatalysts is still a great challenge. Herein, a complex Cu<sub>2</sub>(NO<sub>3</sub>)<sub>4</sub>(BMMB)·H<sub>2</sub>O with a bicopper core is assembled by Cu(NO<sub>3</sub>)<sub>2</sub>·3H<sub>2</sub>O and 1,4-bis{[2-(2’-pyridyl)benzimidazolyl]methyl}benzene (BMMB) for NRA under alkaline conditions. The optimal sample showed excellent nitrate reduction performance with the NO<sub>3</sub><sup>−</sup> conversion rate of 70%, Faradaic efficiency of up to 90%, and NH<sub>3</sub> selectivity of more than 95%. The high-catalytic activity is mainly due to the ingeniously designed copper cores with strong affinity for NO<sub>3</sub><sup>−</sup>, which accelerates the transferring rate of adsorbed nitrate on the Cu surface and increases the efficiency of rate-determining step (NO<sub>3</sub><sup>−</sup> → NO<sub>2</sub><sup>−</sup>) in the whole catalytic process. Therefore, the transformation of surface-exposed nitrate can be rapidly catalyzed by the Cu active sites, facilitating the conversion efficiency of nitrate.
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spelling doaj.art-f9b82d9a69a1469e867c88ad2cd5986a2023-11-24T13:51:05ZengMDPI AGCatalysts2073-43442022-12-011212156110.3390/catal12121561One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to AmmoniaKang-Yu Zeng0Jun-Jie Wang1Xiang Fang2Zuo-Xi Li3Institute of Materials Science and Devices, School of Material Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, ChinaSchool of Chemistry and Chemical Engineering and Anyang Key Laboratory of New Functional Complex Materials, Anyang Normal University, Anyang 455000, ChinaSchool of Chemistry and Chemical Engineering and Anyang Key Laboratory of New Functional Complex Materials, Anyang Normal University, Anyang 455000, ChinaInstitute of Materials Science and Devices, School of Material Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, ChinaAmmonia (NH<sub>3</sub>) plays an irreplaceable role in human life as a promising energy carrier and indispensable chemical raw material. Nitrate electroreduction to ammonium (NRA) not only removes nitrate pollutants, but also can be used for efficient NH<sub>3</sub> production under ambient conditions. However, achieving high efficiency and selectivity of electrocatalysts is still a great challenge. Herein, a complex Cu<sub>2</sub>(NO<sub>3</sub>)<sub>4</sub>(BMMB)·H<sub>2</sub>O with a bicopper core is assembled by Cu(NO<sub>3</sub>)<sub>2</sub>·3H<sub>2</sub>O and 1,4-bis{[2-(2’-pyridyl)benzimidazolyl]methyl}benzene (BMMB) for NRA under alkaline conditions. The optimal sample showed excellent nitrate reduction performance with the NO<sub>3</sub><sup>−</sup> conversion rate of 70%, Faradaic efficiency of up to 90%, and NH<sub>3</sub> selectivity of more than 95%. The high-catalytic activity is mainly due to the ingeniously designed copper cores with strong affinity for NO<sub>3</sub><sup>−</sup>, which accelerates the transferring rate of adsorbed nitrate on the Cu surface and increases the efficiency of rate-determining step (NO<sub>3</sub><sup>−</sup> → NO<sub>2</sub><sup>−</sup>) in the whole catalytic process. Therefore, the transformation of surface-exposed nitrate can be rapidly catalyzed by the Cu active sites, facilitating the conversion efficiency of nitrate.https://www.mdpi.com/2073-4344/12/12/1561electrocatalystscopper complexnitrate affinitynitrate electroreductionammonium production
spellingShingle Kang-Yu Zeng
Jun-Jie Wang
Xiang Fang
Zuo-Xi Li
One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia
Catalysts
electrocatalysts
copper complex
nitrate affinity
nitrate electroreduction
ammonium production
title One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia
title_full One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia
title_fullStr One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia
title_full_unstemmed One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia
title_short One Bicopper Complex with Good Affinity to Nitrate for Highly Selective Electrocatalytic Nitrate Reduction to Ammonia
title_sort one bicopper complex with good affinity to nitrate for highly selective electrocatalytic nitrate reduction to ammonia
topic electrocatalysts
copper complex
nitrate affinity
nitrate electroreduction
ammonium production
url https://www.mdpi.com/2073-4344/12/12/1561
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AT xiangfang onebicoppercomplexwithgoodaffinitytonitrateforhighlyselectiveelectrocatalyticnitratereductiontoammonia
AT zuoxili onebicoppercomplexwithgoodaffinitytonitrateforhighlyselectiveelectrocatalyticnitratereductiontoammonia